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Environmental levels of thallium : Influence of redox properties and anthropogenic sourcesKarlsson, Ulrika January 2006 (has links)
<p>Thallium is a highly toxic element that humans are exposed to mainly by consumption of drinking water and vegetables grown in soil with high thallium content but also through inhalation of particles in the air. Thallium is also present in fossil fuels, alloys, and in electronic utilities. The increasing use of the element and emissions from notably energy production has lead to a higher load on the surface of the Earth. This study aims at increasing the knowledge about the behaviour of thallium in aquatic environments. Focus has been on the redox chemistry of thallium in relation to its mobility, which is of great importance because Tl(I) and Tl(III) have very different properties in this respect.</p><p>The relationship between Tl(I) and Tl(III) in surface waters from contaminated and uncontaminated environments was examined by ion chromatography connected on line to ICP-MS (inductively coupled plasma mass spectrometry). It was found in controlled systems that even though Tl(III) is thermodynamically unstable under fresh water conditions Tl(I) was oxidised in the presence of light and iron(III). This was also confirmed in field studies. When lake water samples were exposed to light, Tl(I) was oxidised and thallium was lost from the solution. The most likely explanation for this was adsorption of thallium to particle surfaces.</p><p>The concentration of thallium in Swedish lakes and soil were measured. In unpolluted lakes the concentration ranges between 4.5-12 ng/l, the sediment concentration was 0.07-1.46 mg/kg. The anthropogenic load was found to have increased since the end of the Second World War although concentrations above background were found since the early industrialisation. In contaminated areas the concentration in soil ranges from 0.64-88 mg/kg, high concentrations were found in systems with alum shale and in soil exposed to runoff from a lead and zinc enrichment plant.</p><p>The mobilisation of thallium from solid phases in contaminated areas was dependent on pH and about 50% of the leachable content was mobilised already at pH 5-6. Once it had been released to water it was highly mobile. These conditions suggest that in a large part of the Swedish environment a high mobility of thallium can be expected.</p>
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Environmental levels of thallium : influence of redox properties and anthropogenic sourcesKarlsson, Ulrika January 2006 (has links)
Thallium is a highly toxic element that humans are exposed to mainly by consumption of drinking water and vegetables grown in soil with high thallium content but also through inhalation of particles in the air. Thallium is also present in fossil fuels, alloys, and in electronic utilities. The increasing use of the element and emissions from notably energy production has lead to a higher load on the surface of the Earth. This study aims at increasing the knowledge about the behaviour of thallium in aquatic environments. Focus has been on the redox chemistry of thallium in relation to its mobility, which is of great importance because Tl(I) and Tl(III) have very different properties in this respect. The relationship between Tl(I) and Tl(III) in surface waters from contaminated and uncontaminated environments was examined by ion chromatography connected on line to ICP-MS (inductively coupled plasma mass spectrometry). It was found in controlled systems that even though Tl(III) is thermodynamically unstable under fresh water conditions Tl(I) was oxidised in the presence of light and iron(III). This was also confirmed in field studies. When lake water samples were exposed to light, Tl(I) was oxidised and thallium was lost from the solution. The most likely explanation for this was adsorption of thallium to particle surfaces. The concentration of thallium in Swedish lakes and soil were measured. In unpolluted lakes the concentration ranges between 4.5-12 ng/l, the sediment concentration was 0.07-1.46 mg/kg. The anthropogenic load was found to have increased since the end of the Second World War although concentrations above background were found since the early industrialisation. In contaminated areas the concentration in soil ranges from 0.64-88 mg/kg, high concentrations were found in systems with alum shale and in soil exposed to runoff from a lead and zinc enrichment plant. The mobilisation of thallium from solid phases in contaminated areas was dependent on pH and about 50% of the leachable content was mobilised already at pH 5-6. Once it had been released to water it was highly mobile. These conditions suggest that in a large part of the Swedish environment a high mobility of thallium can be expected.
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Generation of 4,5-Dihydro-1,2,3-oxadiazole and Study of the Decomposition Products / Erzeugung von 4,5-Dihydro-1,2,3-oxadiazol und Untersuchung der ZersetzungsprodukteSingh, Neeraj 16 December 2015 (has links) (PDF)
4,5-Dihydro-1,2,3-oxadiazoles are postulated to be key intermediates in the synthesis of ketones from alkenes on an industrial scale, alkylation of DNA in vivo, decomposition of N-nitrosoureas (potent carcinogens), and are also a subject of great interest for theoretical chemists. In this thesis, formation of the parent compound and decay into secondary products has been studied by NMR monitoring analysis. The elusive properties and the intermediacy of the parent compound, 4,5-dihydro-1,2,3-oxadiazole, in the decomposition of suitably substituted N-nitrosoureas using Tl(I) alkoxides as bases, have been confirmed by the characterisation of its decay products viz., ethylene oxide, acetaldehyde, and especially diazomethane, at very low temperatures by 1H NMR, 13C NMR, 15N NMR, and relevant 2D NMR methods. Moreover, it has been shown that the methylation of nucleophilic molecules by 3-methyl-4,5-dihydro-1,2,3-oxadiazolium salts, which are considered to be activated forms of β−hydroxyalkylnitrosamines, does not involve 4,5-dihydro-1,2,3-oxadiazole as an intermediate, as has been reported in literature; instead, nucleophilic substitution leading to synthesis of open-chain products dominates the reaction. / 4,5-Dihydro-1,2,3-oxadiazole wurden als Schlüsselintermediate in der industriellen Synthese von Ketonen aus Alkenen, der in vivo Alkylierung von DNA und der Zersetzung von N-Nitrosoharnstoffen (potente Karzinogene) postuliert. Sie sind ebenso von großem Interesse in der theoretischen Chemie. Im Rahmen dieser Arbeit wurde die Bildung der Stammverbindung und deren Zersetzung in sekundäre Produkte mittels NMR-Verfolgung studiert. Die ausgesprochene Kurzlebigkeit der Stammverbindung 4,5-Dihydro-1,2,3-oxadiazol wurde durch die Charakterisierung der Produkte bei der Zersetzung geeignet substituierter N-Nitrosoharnstoffe mit Tl(I)-Alkoxiden bestätigt. Die Zersetzungsprodukte Ethylenoxid, Acetaldehyd und besonders Diazomethan wurden bei sehr niedrigen Temperaturen mittels 1H-NMR, 13C-NMR, 15N-NMR und relevanten 2D-NMR-Methoden charakterisiert.
Des Weiteren konnte gezeigt werden, dass die Methylierung nucleophiler Spezies mit 3-Methyl-4,5-dihydro-1,2,3-oxadiazoliumsalzen, welchen als aktivierte Äquivalente der β−Hydroxyalkylnitrosamine verstanden werden, nicht zur Bildung von 4,5-Dihydro-1,2,3-oxadiazol als Intermediat führt, so wie dies in der Literatur berichtet wurde. Stattdessen wird die Bildung offenkettiger Produkte durch nukleophile Substitution bevorzugt.
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Generation of 4,5-Dihydro-1,2,3-oxadiazole and Study of the Decomposition ProductsSingh, Neeraj 24 November 2015 (has links)
4,5-Dihydro-1,2,3-oxadiazoles are postulated to be key intermediates in the synthesis of ketones from alkenes on an industrial scale, alkylation of DNA in vivo, decomposition of N-nitrosoureas (potent carcinogens), and are also a subject of great interest for theoretical chemists. In this thesis, formation of the parent compound and decay into secondary products has been studied by NMR monitoring analysis. The elusive properties and the intermediacy of the parent compound, 4,5-dihydro-1,2,3-oxadiazole, in the decomposition of suitably substituted N-nitrosoureas using Tl(I) alkoxides as bases, have been confirmed by the characterisation of its decay products viz., ethylene oxide, acetaldehyde, and especially diazomethane, at very low temperatures by 1H NMR, 13C NMR, 15N NMR, and relevant 2D NMR methods. Moreover, it has been shown that the methylation of nucleophilic molecules by 3-methyl-4,5-dihydro-1,2,3-oxadiazolium salts, which are considered to be activated forms of β−hydroxyalkylnitrosamines, does not involve 4,5-dihydro-1,2,3-oxadiazole as an intermediate, as has been reported in literature; instead, nucleophilic substitution leading to synthesis of open-chain products dominates the reaction. / 4,5-Dihydro-1,2,3-oxadiazole wurden als Schlüsselintermediate in der industriellen Synthese von Ketonen aus Alkenen, der in vivo Alkylierung von DNA und der Zersetzung von N-Nitrosoharnstoffen (potente Karzinogene) postuliert. Sie sind ebenso von großem Interesse in der theoretischen Chemie. Im Rahmen dieser Arbeit wurde die Bildung der Stammverbindung und deren Zersetzung in sekundäre Produkte mittels NMR-Verfolgung studiert. Die ausgesprochene Kurzlebigkeit der Stammverbindung 4,5-Dihydro-1,2,3-oxadiazol wurde durch die Charakterisierung der Produkte bei der Zersetzung geeignet substituierter N-Nitrosoharnstoffe mit Tl(I)-Alkoxiden bestätigt. Die Zersetzungsprodukte Ethylenoxid, Acetaldehyd und besonders Diazomethan wurden bei sehr niedrigen Temperaturen mittels 1H-NMR, 13C-NMR, 15N-NMR und relevanten 2D-NMR-Methoden charakterisiert.
Des Weiteren konnte gezeigt werden, dass die Methylierung nucleophiler Spezies mit 3-Methyl-4,5-dihydro-1,2,3-oxadiazoliumsalzen, welchen als aktivierte Äquivalente der β−Hydroxyalkylnitrosamine verstanden werden, nicht zur Bildung von 4,5-Dihydro-1,2,3-oxadiazol als Intermediat führt, so wie dies in der Literatur berichtet wurde. Stattdessen wird die Bildung offenkettiger Produkte durch nukleophile Substitution bevorzugt.
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